Several paramagnetic chemical exchange saturation transfer magnetic resonance imaging (PARACEST MRI) agents for the potential detection of nitric oxide synthase (NOS) have been synthesized and evaluated. These agents are based on an amino acid-or dipeptide-decorated DOTAM (1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid amide) chelator possessing either Tm3+ or Dy3+. The amino acid and dipeptide decorated DOTAMs were designed such that the terminal amino acid pendant group was l-arginine, which may be converted to l-citrulline by NOS. Preliminary evaluation has revealed that some of the l-arginine-decorated complexes are recognized and metabolized by the NOS. Differences in the CEST properties between Dy3+-metallated l-arginine-and l-citrulline-modified complexes suggest that these might be suitable for imaging of the NOS enzymatic activity.